Abstract A novel convenient room-temperature method for surface covering of carbon nanotubes (CNTs) with few-layer MoS2 shell was developed. For this purpose, liquid-phase single-layer dispersions of molybdenum disulfide produced by chemical exfoliation of its compound with lithium, LiMoS2, were applied. As evidenced by XRD and TEM studies, the dispersed MoS2 layers readily attach to the outer CNT surface and tend to envelop it. Measuring the interlayer distances in the vicinity of the MoS2-CNT interface showed, that deposited particles typically contain 1-3 (rarely, up to 10) MoS2 layers, which are in close contact with graphitic CNT walls. Similar deposition performed in the presence of cationic polymers containing polydiallyldimethylammonium units was found to lead to incorporation of polymer molecules in the sulfide shell of CNT in the form of 0.5 nm thick organic interlayers between the layers of MoS2. The same sequence of the layers of MoS2 and the polymer is also realized in the absence of CNT due to self-organization of the components. The method presented in this work has a great potential for designing other nanohybrid structures with participation of layered metal sulfides.